A new layered mixed-linker metal organic framework [Zn-2(iso)(2)(pcih)(2)](n) (MOF) built from isophthalate ions (iso(2-)) and 4-pyridinecarbaldehyde isonicotinoyl hydrazone (pcih) was prepared using both solution and mechanochemical methods. By use of the latter, the 2D MOF is obtained either in a one-mortar three-component grinding or on the way of a two-step mechanosynthesis. Tuning of mechanochemical synthetic conditions allowed 118 to identify both necessary and favorable factors for the solid-state formation of the MOF. Single-crystal X-ray diffraction reveals the presence of interdigitated layers in the ABAB. arrangement and interlayer OD cavities-filled With ::guest molecules. Upon thermal activation, the dynamic framework exhibits stepwise and selective adsorption of CO2 over N-2 as well as high-pressure H-2 adsorption reaching maximum excess of 1.15 wt% at 77 K. The mechanochemical synthetic protocol is expanded to a few other interdigitated structures.